Title: Cesium-Coated Halide Perovskites as a Photocathode Material: Modeling Insights

Abstract

Photocathodes emit electrons when illuminated, a process utilized across many technologies. Cutting-edge applications require a set of operating conditions that are not met with current photocathode materials. Meanwhile, halide perovskites have been studied extensively and have shown a lot of promise for a wide variety of optoelectronic applications. Well-documented halide perovskite properties such as inexpensive growth techniques, improved carrier mobility, low trap density, and tunable direct band gaps make them promising candidates for next-generation photocathode materials. In this study, we use density functional theory to explore the possible application of pure inorganic perovskites (CsPbBr₃ and CsPbI₃) as photocathodes. It is determined that the addition of a Cs coating improved the performance by lowering the work function anywhere between 1.5 and 3 eV depending on the material, crystal surface, and surface coverage. A phenomenological model, modified from that developed by Gyftopoulos and Levine, is used to predict the reduction in work function with Cs coverage. The results of this work aim to guide the further experimental development of Cs-coated halide perovskites for photocathode materials.

Authors:

Lewis, Sina G. ^[1]; Ghosh, Dibyajyoti  ^[2];

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• Search DOE PAGES for ORCID "0000-0002-3640-7537"

Jensen, Kevin L. ^[3]; Finkenstadt, Daniel ^[4]; Shabaev, Andrew ^[3]; Lambrakos, Samuel G. ^[3]; Liu, Fangze  ^[2];

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• Search DOE PAGES for ORCID "0000-0003-3114-5280"

Nie, Wanyi  ^[2];

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• Search DOE PAGES for ORCID "0000-0002-5909-3155"

Blancon, Jean-Christophe ^[5]; Zhou, Liujiang  ^[6];

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• Search DOE PAGES for ORCID "0000-0001-5814-4486"

Crochet, Jared J.  ^[2];

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• Search DOE PAGES for ORCID "0000-0002-9570-2173"

Moody, Nathan  ^[2];

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• Search DOE PAGES for ORCID "0000-0001-6568-7841"

Mohite, Aditya D.  ^[5];

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• Search DOE PAGES for ORCID "0000-0001-8865-409X"

Tretiak, Sergei  ^[2];

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• Search DOE PAGES for ORCID "0000-0001-5547-3647"

Neukirch, Amanda J.  ^[2]

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• Search DOE PAGES for ORCID "0000-0002-6583-0086"

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+ Show Author Affiliations

1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Colorado, Boulder, CO (United States)
2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
3. Naval Research Lab. (NRL), Washington, DC (United States)
4. US Naval Academy, Annapolis, MD (United States)
5. Rice Univ., Houston, TX (United States)
6. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Electronic Science and Technology of China, Chengdu (China)

Publication Date:

Thu Jul 01 00:00:00 EDT 2021

Research Org.:

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:

USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:

1822813

Report Number(s):

LA-UR-21-24212
Journal ID: ISSN 1948-7185; TRN: US2214514

Grant/Contract Number:  

89233218CNA000001

Resource Type:

Accepted Manuscript

Journal Name:

Journal of Physical Chemistry Letters

Additional Journal Information:

Journal Volume: 12; Journal Issue: 27; Journal ID: ISSN 1948-7185

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; coating materials; work function; photonics; perovskites; materials